Precision Chemistry最新文献_第8页

Molecular Interactions in Atomically Precise Metal Nanoclusters 原子精度金属纳米团簇中的分子相互作用

Precision Chemistry Pub Date : 2024-08-22 DOI: 10.1021/prechem.4c0004410.1021/prechem.4c00044

Jing Qian, Zhucheng Yang, Jingkuan Lyu, Qiaofeng Yao* and Jianping Xie*,

{"title":"Molecular Interactions in Atomically Precise Metal Nanoclusters","authors":"Jing Qian, Zhucheng Yang, Jingkuan Lyu, Qiaofeng Yao* and Jianping Xie*, ","doi":"10.1021/prechem.4c0004410.1021/prechem.4c00044","DOIUrl":"https://doi.org/10.1021/prechem.4c00044https://doi.org/10.1021/prechem.4c00044","url":null,"abstract":"For nanochemistry, precise manipulation of nanoscale structures and the accompanying chemical properties at atomic precision is one of the greatest challenges today. The scientific community strives to develop and design customized nanomaterials, while molecular interactions often serve as key tools or probes for this atomically precise undertaking. In this Perspective, metal nanoclusters, especially gold nanoclusters, serve as a good platform for understanding such nanoscale interactions. These nanoclusters often have a core size of about 2 nm, a defined number of core metal atoms, and protecting ligands with known crystal structure. The atomically precise structure of metal nanoclusters allows us to discuss how the molecular interactions facilitate the systematic modification and functionalization of nanoclusters from their inner core, through the ligand shell, to the external assembly. Interestingly, the atomic packing structure of the nanocluster core can be affected by forces on the surface. After discussing the core structure, we examine various atomic-level strategies to enhance their photoluminescent quantum yield and improve nanoclusters’ catalytic performance. Beyond the single cluster level, various attractive or repulsive molecular interactions have been employed to engineer the self-assembly behavior and thus packing morphology of metal nanoclusters. The methodological and fundamental insights systemized in this review should be useful for customizing the cluster structure and assembly patterns at the atomic level.","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 10","pages":"495–517 495–517"},"PeriodicalIF":0.0,"publicationDate":"2024-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00044","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550697","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Quadruple[6]Helicene Featuring Pyrene Core: Unraveling Contorted Aromatic Core with Larger Effective Conjugation 以芘为核心的四[6]联苯：以更大的有效共轭解开扭曲的芳香族核心

Precision Chemistry Pub Date : 2024-08-13 DOI: 10.1021/prechem.4c0003810.1021/prechem.4c00038

Christopher Wallerius, Otgonbayar Erdene-Ochir, Eva Van Doeselar, Ronald Alle, Anh Tu Nguyen, Marvin F. Schumacher, Arne Lützen, Klaus Meerholz and Sai Ho Pun*,

{"title":"Quadruple[6]Helicene Featuring Pyrene Core: Unraveling Contorted Aromatic Core with Larger Effective Conjugation","authors":"Christopher Wallerius, Otgonbayar Erdene-Ochir, Eva Van Doeselar, Ronald Alle, Anh Tu Nguyen, Marvin F. Schumacher, Arne Lützen, Klaus Meerholz and Sai Ho Pun*, ","doi":"10.1021/prechem.4c0003810.1021/prechem.4c00038","DOIUrl":"https://doi.org/10.1021/prechem.4c00038https://doi.org/10.1021/prechem.4c00038","url":null,"abstract":"Multiple helicenes display distinct aromatic cores characterized by highly twisted rings that are shared or fused with constituent helicene moieties. Diversifying these aromatic cores unlocks avenues for creating multiple helicenes with distinct properties and topologies. Herein we report the synthesis of a quadruple[6]helicene featuring pyrene as the aromatic core. The synthesis involved key steps of the annulative π-extension reaction and Scholl reaction. By extending multiple helicenes along the axial direction, the degree of contortion of the aromatic core can be controlled from nearly flat to highly twisted. Notably, quadruple[6]helicene exhibits a significant red-shift of 0.49 eV compared to quadruple[4]helicenes, of which the red-shift arises from both π-extension and augmented effective conjugation due to enhanced twisting. Quantum chemical calculations demonstrate that the degree of contortion in the pyrene core adeptly governs the energy levels of the HOMO and LUMO, which offers an alternative strategy beyond mere enlargement of the π backbone. An intriguing serendipitous finding reveals the formation of one-molecule-thick supramolecular homochiral nanosheets through self-interlocking interactions of enantiomers in single crystals, a rare packing motif for multiple helicenes.","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 9","pages":"488–494 488–494"},"PeriodicalIF":0.0,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00038","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276208","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Quadruple[6]Helicene Featuring Pyrene Core: Unraveling Contorted Aromatic Core with Larger Effective Conjugation. 以芘为核心的四[6]联苯：以更大的有效共轭解开扭曲的芳香族核心。

Precision Chemistry Pub Date : 2024-08-13 eCollection Date: 2024-09-23 DOI: 10.1021/prechem.4c00038

Christopher Wallerius, Otgonbayar Erdene-Ochir, Eva Van Doeselar, Ronald Alle, Anh Tu Nguyen, Marvin F Schumacher, Arne Lützen, Klaus Meerholz, Sai Ho Pun

{"title":"Quadruple[6]Helicene Featuring Pyrene Core: Unraveling Contorted Aromatic Core with Larger Effective Conjugation.","authors":"Christopher Wallerius, Otgonbayar Erdene-Ochir, Eva Van Doeselar, Ronald Alle, Anh Tu Nguyen, Marvin F Schumacher, Arne Lützen, Klaus Meerholz, Sai Ho Pun","doi":"10.1021/prechem.4c00038","DOIUrl":"https://doi.org/10.1021/prechem.4c00038","url":null,"abstract":"Multiple helicenes display distinct aromatic cores characterized by highly twisted rings that are shared or fused with constituent helicene moieties. Diversifying these aromatic cores unlocks avenues for creating multiple helicenes with distinct properties and topologies. Herein we report the synthesis of a quadruple[6]helicene featuring pyrene as the aromatic core. The synthesis involved key steps of the annulative π-extension reaction and Scholl reaction. By extending multiple helicenes along the axial direction, the degree of contortion of the aromatic core can be controlled from nearly flat to highly twisted. Notably, quadruple[6]helicene exhibits a significant red-shift of 0.49 eV compared to quadruple[4]helicenes, of which the red-shift arises from both π-extension and augmented effective conjugation due to enhanced twisting. Quantum chemical calculations demonstrate that the degree of contortion in the pyrene core adeptly governs the energy levels of the HOMO and LUMO, which offers an alternative strategy beyond mere enlargement of the π backbone. An intriguing serendipitous finding reveals the formation of one-molecule-thick supramolecular homochiral nanosheets through self-interlocking interactions of enantiomers in single crystals, a rare packing motif for multiple helicenes.","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 9","pages":"488-494"},"PeriodicalIF":0.0,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11501045/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142547977","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Precision Control of Amphoteric Doping in Cu _x Bi₂Se₃ Nanoplates. Cu x Bi2Se3 纳米板中两性掺杂的精确控制。

Precision Chemistry Pub Date : 2024-08-04 eCollection Date: 2024-08-26 DOI: 10.1021/prechem.4c00046

Huaying Ren, Jingxuan Zhou, Ao Zhang, Zixi Wu, Jin Cai, Xiaoyang Fu, Jingyuan Zhou, Zhong Wan, Boxuan Zhou, Yu Huang, Xiangfeng Duan

{"title":"Precision Control of Amphoteric Doping in Cu x Bi2Se3 Nanoplates.","authors":"Huaying Ren, Jingxuan Zhou, Ao Zhang, Zixi Wu, Jin Cai, Xiaoyang Fu, Jingyuan Zhou, Zhong Wan, Boxuan Zhou, Yu Huang, Xiangfeng Duan","doi":"10.1021/prechem.4c00046","DOIUrl":"10.1021/prechem.4c00046","url":null,"abstract":"Copper-doped Bi2Se3 (Cu x Bi2Se3) is of considerable interest for tailoring its electronic properties and inducing exotic charge correlations while retaining the unique Dirac surface states. However, the copper dopants in Cu x Bi2Se3 display complex electronic behaviors and may function as either electron donors or acceptors depending on their concentration and atomic sites within the Bi2Se3 crystal lattice. Thus, a precise understanding and control of the doping concentration and sites is of both fundamental and practical significance. Herein, we report a solution-based one-pot synthesis of Cu x Bi2Se3 nanoplates with systematically tunable Cu doping concentrations and doping sites. Our studies reveal a gradual evolution from intercalative sites to substitutional sites with increasing Cu concentrations. The Cu atoms at intercalative sites function as electron donors while those at the substitutional sites function as electron acceptors, producing distinct effects on the electronic properties of the resulting materials. We further show that Cu0.18Bi2Se3 exhibits superconducting behavior, which is not present in Bi2Se3, highlighting the essential role of Cu doping in tailoring exotic quantum properties. This study establishes an efficient methodology for precise synthesis of Cu x Bi2Se3 with tailored doping concentrations, doping sites, and electronic properties.","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 8","pages":"421-427"},"PeriodicalIF":0.0,"publicationDate":"2024-08-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11351425/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142112793","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Precision Control of Amphoteric Doping in CuxBi2Se3 Nanoplates CuxBi2Se3 纳米板中两性掺杂的精确控制

Precision Chemistry Pub Date : 2024-08-04 DOI: 10.1021/prechem.4c0004610.1021/prechem.4c00046

Huaying Ren, Jingxuan Zhou, Ao Zhang, Zixi Wu, Jin Cai, Xiaoyang Fu, Jingyuan Zhou, Zhong Wan, Boxuan Zhou, Yu Huang and Xiangfeng Duan*,

{"title":"Precision Control of Amphoteric Doping in CuxBi2Se3 Nanoplates","authors":"Huaying Ren, Jingxuan Zhou, Ao Zhang, Zixi Wu, Jin Cai, Xiaoyang Fu, Jingyuan Zhou, Zhong Wan, Boxuan Zhou, Yu Huang and Xiangfeng Duan*, ","doi":"10.1021/prechem.4c0004610.1021/prechem.4c00046","DOIUrl":"https://doi.org/10.1021/prechem.4c00046https://doi.org/10.1021/prechem.4c00046","url":null,"abstract":"Copper-doped Bi2Se3 (CuxBi2Se3) is of considerable interest for tailoring its electronic properties and inducing exotic charge correlations while retaining the unique Dirac surface states. However, the copper dopants in CuxBi2Se3 display complex electronic behaviors and may function as either electron donors or acceptors depending on their concentration and atomic sites within the Bi2Se3 crystal lattice. Thus, a precise understanding and control of the doping concentration and sites is of both fundamental and practical significance. Herein, we report a solution-based one-pot synthesis of CuxBi2Se3 nanoplates with systematically tunable Cu doping concentrations and doping sites. Our studies reveal a gradual evolution from intercalative sites to substitutional sites with increasing Cu concentrations. The Cu atoms at intercalative sites function as electron donors while those at the substitutional sites function as electron acceptors, producing distinct effects on the electronic properties of the resulting materials. We further show that Cu0.18Bi2Se3 exhibits superconducting behavior, which is not present in Bi2Se3, highlighting the essential role of Cu doping in tailoring exotic quantum properties. This study establishes an efficient methodology for precise synthesis of CuxBi2Se3 with tailored doping concentrations, doping sites, and electronic properties.","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 8","pages":"421–427 421–427"},"PeriodicalIF":0.0,"publicationDate":"2024-08-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00046","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142075377","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Pd-Catalyzed Stereospecific Glycosyl Cross-Coupling of Reversed Anomeric Stannanes for Modular Synthesis of Nonclassical C-Glycosides 钯催化反向同分异构锡烷的立体特异性糖基交叉偶联用于非经典 C-糖苷的模块化合成

Precision Chemistry Pub Date : 2024-07-21 DOI: 10.1021/prechem.4c0004210.1021/prechem.4c00042

Guoqiang Cheng, Bo Yang, Yang Han, Wei Lin, Siyuan Tao, Yong Nian*, Yingzi Li*, Maciej A. Walczak and Feng Zhu*,

{"title":"Pd-Catalyzed Stereospecific Glycosyl Cross-Coupling of Reversed Anomeric Stannanes for Modular Synthesis of Nonclassical C-Glycosides","authors":"Guoqiang Cheng, Bo Yang, Yang Han, Wei Lin, Siyuan Tao, Yong Nian*, Yingzi Li*, Maciej A. Walczak and Feng Zhu*, ","doi":"10.1021/prechem.4c0004210.1021/prechem.4c00042","DOIUrl":"https://doi.org/10.1021/prechem.4c00042https://doi.org/10.1021/prechem.4c00042","url":null,"abstract":"Nonclassical C-glycosides, distinguished by their unique glycosidic bond connection mode, represent a promising avenue for the development of carbohydrate-based drugs. However, the accessibility of nonclassical C-glycosides hinders broader investigations into their structural features and modes of action. Herein, we present the first example of Pd-catalyzed stereospecific glycosylation of nonclassical anomeric stannanes with aryl or vinyl halides. This method furnishes desired nonclassical aryl and vinyl C-glycosides in good to excellent yields, while allowing for exclusive control of nonclassical anomeric configuration. Of significant note is the demonstration of the generality and practicality of this nonclassical C-glycosylation approach across more than 50 examples, encompassing various protected and unprotected saccharides, deoxy sugars, oligopeptides, and complex molecules. Furthermore, biological evaluation indicates that nonclassical C-glycosylation modifications of drug molecules can positively impact their biological activity. Additionally, extensive computational studies are conducted to elucidate the rationale behind differences in reaction reactivity, unveiling a transmetalation transition state containing silver (Ag) within a six-membered ring. Given its remarkable controllability, predictability, and consistently high chemical selectivity and stereospecificity regarding nonclassical anomeric carbon and Z/E configuration, the method outlined in this study offers a unique solution to the longstanding challenge of accessing nonclassical C-glycosides with exclusive stereocontrol.","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 11","pages":"587–599 587–599"},"PeriodicalIF":0.0,"publicationDate":"2024-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00042","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694446","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Pd-Catalyzed Stereospecific Glycosyl Cross-Coupling of Reversed Anomeric Stannanes for Modular Synthesis of Nonclassical C-Glycosides 钯催化反向同分异构锡烷的立体特异性糖基交叉偶联用于非经典 C-糖苷的模块化合成

Precision Chemistry Pub Date : 2024-07-21 DOI: 10.1021/prechem.4c00042

Guoqiang Cheng, Bo-Wen Yang, Yang Han, Wei Lin, Siyuan Tao, Yong Nian, Yingzi Li, M. Walczak, Feng Zhu

引用次数: 0

Reducing Energy Costs during Hydrogen Production from Water Electrolysis by Coupling Small Molecule Oxidation: From Molecular Catalysis to Industrial Exploration 通过耦合小分子氧化降低水电解制氢过程中的能源成本：从分子催化到工业探索

Precision Chemistry Pub Date : 2024-07-01 DOI: 10.1021/prechem.4c0002510.1021/prechem.4c00025

Jia Cheng, Yang Xiang, Xun Huang* and Zidong Wei*,

{"title":"Reducing Energy Costs during Hydrogen Production from Water Electrolysis by Coupling Small Molecule Oxidation: From Molecular Catalysis to Industrial Exploration","authors":"Jia Cheng, Yang Xiang, Xun Huang* and Zidong Wei*, ","doi":"10.1021/prechem.4c0002510.1021/prechem.4c00025","DOIUrl":"https://doi.org/10.1021/prechem.4c00025https://doi.org/10.1021/prechem.4c00025","url":null,"abstract":"Hydrogen energy has garnered significant attention in recent years as a solution to address the global energy crisis and environmental pollution. While water electrolysis stands out as the most promising method to produce green hydrogen, the sluggish reaction kinetics of the oxygen evolution reaction (OER) on the anode increases the cost of hydrogen production. One potential solution to this challenge is replace OER with the thermodynamically more favorable oxidation of small molecules, which can efficiently reduce the energy cost while simultaneously yielding high-value chemicals. Up to now, various organic oxidation reactions have been reported to couple with hydrogen evolution, including alcohol oxidation, biomass platform molecule upgrading, and sacrificial reagents oxidation associated with wastewater treatments. This review concentrates on the recent advancements in the mechanism, catalyst, reactor, and process in this field, with a discussion on its prospects for commercialization.","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"2 9","pages":"447–470 447–470"},"PeriodicalIF":0.0,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00025","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276267","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Reducing Energy Costs during Hydrogen Production from Water Electrolysis by Coupling Small Molecule Oxidation: From Molecular Catalysis to Industrial Exploration 通过耦合小分子氧化降低水电解制氢过程中的能源成本：从分子催化到工业探索

Precision Chemistry Pub Date : 2024-07-01 DOI: 10.1021/prechem.4c00025

Jia Cheng, Yang Xiang, Xun Huang, Zidong Wei

引用次数: 0

Porphyrin/Fullerene Porous Molecular Cocrystal Featuring a Robust One-Dimensional Channel 具有稳健一维通道的卟啉/富勒烯多孔分子共晶体

Precision Chemistry Pub Date : 2024-06-12 DOI: 10.1021/prechem.4c00036

Nobuhiro Sato, Ryojun Toyoda, Tetsu Sato, Zi Lang Goo, S. Takaishi, Koki Chida, Takeharu Yoshii, Hirotomo Nishihara, K. Sugimoto, Ryota Sakamoto

引用次数: 0